General Quantum Alchemical Free Energy Simulations via Hamiltonian Interpolation
Uloženo v:
| Název: | General Quantum Alchemical Free Energy Simulations via Hamiltonian Interpolation |
|---|---|
| Autoři: | Chenghan Li, Xing Zhang, Garnet Kin-Lic Chan |
| Zdroj: | Journal of Chemical Theory and Computation. 21:6644-6652 |
| Publication Status: | Preprint |
| Informace o vydavateli: | American Chemical Society (ACS), 2025. |
| Rok vydání: | 2025 |
| Témata: | Chemical Physics (physics.chem-ph), Biological Physics (physics.bio-ph), Physics - Chemical Physics, FOS: Physical sciences, Physics - Biological Physics |
| Popis: | We present an implementation of alchemical free energy simulations at the quantum mechanical level by directly interpolating the electronic Hamiltonian. The method is compatible with any level of electronic structure theory and requires only one quantum calculation for each molecular dynamics step in contrast to multiple energy evaluations that would be needed when interpolating the ground-state energies. We demonstrate the correctness and applicability of the technique by computing alchemical free energy changes of gas-phase molecules, with both nuclear and electron creation/annihilation. We also show an initial application to first-principles pKa calculation for solvated molecules where we quantum mechanically annihilate a bonded proton. |
| Druh dokumentu: | Article |
| Jazyk: | English |
| ISSN: | 1549-9626 1549-9618 |
| DOI: | 10.1021/acs.jctc.5c00682 |
| DOI: | 10.48550/arxiv.2408.17002 |
| Přístupová URL adresa: | http://arxiv.org/abs/2408.17002 |
| Rights: | STM Policy #29 CC BY |
| Přístupové číslo: | edsair.doi.dedup.....ae49a0cc19c8a0f06d49bf04dc722288 |
| Databáze: | OpenAIRE |
Nájsť tento článok vo Web of Science | Abstrakt: | We present an implementation of alchemical free energy simulations at the quantum mechanical level by directly interpolating the electronic Hamiltonian. The method is compatible with any level of electronic structure theory and requires only one quantum calculation for each molecular dynamics step in contrast to multiple energy evaluations that would be needed when interpolating the ground-state energies. We demonstrate the correctness and applicability of the technique by computing alchemical free energy changes of gas-phase molecules, with both nuclear and electron creation/annihilation. We also show an initial application to first-principles pKa calculation for solvated molecules where we quantum mechanically annihilate a bonded proton. |
|---|---|
| ISSN: | 15499626 15499618 |
| DOI: | 10.1021/acs.jctc.5c00682 |